A twin column cyclic process for the preparation of 239 Devices and methods for np tracer

Abstract

This invention relates to a dual-column cyclic preparation method. 239 The apparatus and method for Np tracers belong to the field of actinide isotope separation and preparation technology, and solve the problem of... 239 The technical challenges of low purity and unstable recovery rates in Np tracer preparation are addressed by this device, which includes a temperature controller, a radiation shield, a storage tank unit, a chromatography separation unit, a waste liquid collector, a product collector, valves, and a transfer pump. Liquid from the storage tank unit is pumped into the chromatography separation unit, and liquid exiting the chromatography separation unit enters either the waste liquid collector or the product collector. The chromatography separation unit includes a TODGA chromatography adsorption column and LN or P... 204 or P 507 Chromatographic adsorption column. The method includes preparing a feed solution, washing solution, eluent, and chromatographic adsorption column before separation; adsorption, washing, and elution steps for neptunium. This invention is used for preparing... 239 Np tracer.

Description

Technical Field

[0001] This invention belongs to the field of actinide isotope separation and preparation technology, specifically relating to a dual-column cyclic preparation method. 239 Apparatus and method for Np tracers. Background Technology

[0002] 239 Np has a half-life of 2.35 days and is a short-lived gamma radionuclide, often used in environmental samples as a long-lived actinide alpha radionuclide. 237 Np (half-life 2.14 × 10⁻⁶) 6 A tracer for the recovery rate of chemical separation processes in the analysis (year). It can be produced in two ways: the first method uses... 238 U neutron activation reaction generates 239 U (half-life 23.5 minutes), 239 U quickly passed β - decay generation 239 Np, this method not only requires expensive neutron source irradiation equipment, but also needs to solve a large number of target nuclei 238 U, fission products and 239 The isolation of Np is not commonly used in laboratories. The second method is the parent nuclide. 243 Am (half-life 7370 years) produces daughter cells through its own alpha decay. 239 Np. Due to the parent nuclide 243 Am has a half-life much longer than its daughter nuclides. 239 Np, therefore, undergoes a certain daughter nucleus half-life. 243 Am can generate a certain level of activity. 239 Np can be used to isolate and extract newly formed daughter nuclides from the parent nucleus. This method is a "milking the cow" preparation method and is currently commonly used in laboratories. 239 Np tracer preparation method.

[0003] Extraction chromatography, due to its combination of the high selectivity of solvent extraction and the high efficiency of chromatography, is often used in... 239 Preparation of Np tracers. (Reference: Reich et al. Extraction chromatography for the separation of...) 239 Npfrom 243 Am.J Radioanal Nucl Chem. 2005, 266(1):71-74) reported a method based on the principle of ferrous aminosulfonate reduction, using an Aliquat-336 silica gel column to extract tetravalent neptunium and separate trivalent americium. However, the neptunium contained not only 0.5% americium contamination, but also the recovered neptunium... 243The Am mother liquor contains impurities such as Fe ions introduced during the reduction process, requiring additional steps to remove these interfering substances before proceeding to the next step. 239 The preparation of Np is very inconvenient. (Patent ZL 201310626323.7 Shi Yanmei et al. A method...) 239 The reported method for rapid preparation of Np tracers is relatively simple, but the recovery... 243 Am mother liquor medium and the next 239 The inconsistency in the column loading medium required for Np preparation necessitates lengthy transfer steps such as evaporation, conversion, and re-dissolution before it can be used for the next preparation, inevitably leading to... 243 The method suffers from Am loss, and since it does not control the valence state of neptunium, it is difficult to guarantee [the safety of the method]. 239 Stability and reproducibility of Np tracer recovery.

[0004] because 239 Np has a short half-life, and each preparation... 239 Np tracers decay rapidly. Therefore, frequent, periodic "milking" preparations are necessary to meet the requirements for routine, multi-batch sample preparation. 237 The need for Np analysis necessitates that the processes, both in the initial preparation and in subsequent preparations, be simpler and easier to implement, while ensuring sufficiently high purity and recovery rates for both the parent and daughter products. Clearly, the methods described above do not adequately meet current technological requirements. Summary of the Invention

[0005] In order to overcome 239 The preparation of Np tracers suffers from drawbacks such as low purity of the parent and daughter molecules and unstable recovery rates. This invention proposes a dual-column cyclic preparation method. 239 Apparatus and method for Np tracers.

[0006] The technical solution adopted by this invention to solve its technical problem is:

[0007] A dual-column cyclic preparation 239 The device for Np tracers includes a temperature controller, a radiation shield, a liquid storage tank unit, a chromatography separation unit, a waste liquid collector, a product collector, valves, a delivery pump, and piping.

[0008] The aforementioned temperature controller is a constant temperature electric heating mantle, an electric heating belt, or a water bath, placed around the outside of a storage tank containing americium-neptunium radioactive solution.

[0009] The aforementioned radiation shield is made of lead bricks or lead-containing materials and is placed around the thermostat.

[0010] The aforementioned liquid storage tank unit, color layer separation unit, waste liquid collector, valve, and product collector are connected by pipelines;

[0011] The above-mentioned liquid storage tank unit includes a material liquid storage tank, a washing liquid storage tank, a first-stage rinsing liquid storage tank, a second-stage rinsing liquid storage tank, and a third-stage rinsing liquid storage tank.

[0012] The aforementioned chromatography separation unit includes a TODGA chromatography adsorption column and LN or P 204 or P 507 Chromatographic adsorption column;

[0013] The bottom of the liquid storage tank is connected to the inlet of the delivery pump via pipes and valves; the outlets of the washing liquid storage tank, the first-stage rinsing liquid storage tank, the second-stage rinsing liquid storage tank, and the third-stage rinsing liquid storage tank are connected to the inlet of the delivery pump via valves.

[0014] The outlet of the delivery pump is connected to the TODGA chromatograph and LN or P column, respectively. 204 or P 507 Connection to the feed inlet of the chromatography column;

[0015] The outlet of the aforementioned TODGA chromatography column is connected to a waste liquid collector, LN, or P via valves. 204 or P 507 The inlet of the chromatography column is connected to the product collector;

[0016] The above LN or P 204 or P 507 The outlet of the chromatography-adsorption column is connected to a waste liquid collector and a storage tank containing americium-neptunium radioactive solution via valves.

[0017] The aforementioned piping uses silicone tubing; the valves are solenoid valves; and the transfer pump is a peristaltic pump. This allows for microcomputer control of the solenoid valves and peristaltic pump, enabling automatic control of the separation process and reducing the impact of radioactive nuclide radiation and toxicity on the human body. The peristaltic pump uses a flexible tubing compression method to deliver the separation liquid, and the flow rate and velocity of the liquid are controlled by the pump's rotation speed.

[0018] A dual-column cyclic preparation 239 The method for using Np tracers includes the following steps:

[0019] Step 1: Preparation before separation

[0020] Add 100 mg of sodium nitrite to the radioactive solution containing americium, keep it at a constant temperature of 70-100 degrees Celsius for 15 minutes, and then cool it to form the feed solution before separation.

[0021] The acid is dissolved in water to form an aqueous detergent and an aqueous rinsing solution.

[0022] TODGA, LN, or P 204 or P 507 The resins were separately packed into the color layer columns;

[0023] Step 2: Adsorption of americium-neptunium

[0024] The aqueous radioactive solution containing americium and neptunium prepared in step one was passed through a TODGA chromatography column to adsorb americium and neptunium, and the effluent was collected as waste liquid.

[0025] Step 3: Washing

[0026] The washing solution is washed through a TODGA chromatography column, and the effluent is collected as waste liquid.

[0027] Step 4: Rinse

[0028] The first-stage eluent is used to desorb neptunium using a TODGA chromatography column; the effluent, which is a radioactive solution of neptunium, is collected in a product collector.

[0029] The second-stage eluent is sequentially passed through a TODGA chromatography column and LN or P... 204 or P 507 The americium is desorbed and re-adsorbed using a chromatography column, and the effluent is collected as waste liquid.

[0030] The first-stage rinsing solution passes through LN or P 204 or P 507 The chromatography column is washed, and the effluent is collected as waste liquid.

[0031] Washing solution via LN or P 204 or P 507 The americium is desorbed by a chromatography column, and the effluent, which is a radioactive americium solution, is collected in a storage tank for americium-neptunium radioactive solution.

[0032] Step 5: Regeneration

[0033] The third-stage eluent is passed through a TODGA chromatography column, and the effluent is collected as waste liquid.

[0034] The second-stage rinsing solution is passed through LN or P. 204 or P 507 The pipeline between the chromatography adsorption column and the TODGA chromatography adsorption column is used to collect the effluent as waste liquid.

[0035] The second-stage rinsing solution is passed through LN or P. 204 or P 507 Chromatographic adsorption column, the effluent is collected as waste liquid;

[0036] The washing liquid is passed through a TODGA chromatography column, and the effluent is collected as waste liquid.

[0037] Step Six: Recycle

[0038] After the americium solution in the americium-naphthene radioactive solution storage tank is left for 7-8 days, a sufficient amount of new americium will be generated. 239Np, repeat steps one through five to proceed to the next preparation process, and repeat this process cyclically. 239 Np tracer.

[0039] The aforementioned radioactive solution of americium-neptunium is rich in sodium nitrite. 243 Am and its decay products 239 A solution composed of Np.

[0040] The acid in step 1 above is nitric acid and hydrochloric acid, hydrofluoric acid, or a combination of the above acids, and the concentration of the acid is from 0.01 to 8.0 mol / L.

[0041] The radioactive solution containing americium-neptunium is 4-8 mol / L HNO3; the aqueous washing solution is 4-8 mol / L HNO3 solution; the first-stage rinsing solution is 0.01-0.5 mol / L HNO3 solution; the second-stage rinsing solution is 0.05-0.2 mol / L HCl solution; and the third-stage rinsing solution is 0.05-0.2 mol / L HCl solution containing 0.05-0.5 mol / L HF.

[0042] The above TODGA color layer columns and LN or P 204 or P 507 Chromatography columns can be automatically regenerated for use in the next preparation process.

[0043] The above-mentioned preparation after the first separation 239 After Np, the recovered americium radioactive solution has the same acid composition and concentration as the americium-neptunium radioactive solution required before preparation, and is ready for the next preparation.

[0044] The above-mentioned preparation cycle is repeated 10 times, after which the chromatography adsorption column needs to be replaced.

[0045] The americium recovered from the separation was stored in a storage tank, rather than on a chromatography column.

[0046] The aforementioned americium-neptene radioactive solution storage tank is shielded on the outside.

[0047] The above separation and preparation process was carried out at room temperature.

[0048] The beneficial effects of this invention are:

[0049] A dual-column cyclic preparation 239 The Np tracer device effectively utilizes the adsorption properties of americium and neptunium by two chromatography columns, cleverly matching the input and output solutions between the two columns to enable the preparation of high-purity TODGA chromatography-adsorption columns. 239 Np tracer, LN or P 204 or P 507 Chromatographic adsorption column conversion 243The Am solution system serves as the starting material medium, laying the foundation for automated process control and cyclic preparation.

[0050] A dual-column cyclic preparation 239 Device for recovering Np tracers 243 The Am solution is automatically stored in a radiation-shielded reservoir instead of being retained on the chromatography column, which avoids the radiation degradation of the organic adsorbent material, effectively ensuring the multiple recycling of the chromatography column, and at the same time ensuring the safety of personnel from radiation exposure.

[0051] A dual-column cyclic preparation 239 The method for Np tracers features clearly defined functions for each separation unit, a simple process that is easy to control and adjust, and an integrated design encompassing separation, purification, preparation, media switching, and regeneration. The entire process can be completed within 1.5 hours and can be replicated up to ten times. 239 Cyclic preparation of Np tracers.

[0052] A dual-column cyclic preparation 239 Compared with existing methods, the Np tracer method achieves automated separation of americium and neptunium under programmed control; 239 Np and 243 The recovery rate of Am was better than 95% and 99%. 239 The Np radioactivity purity reached 99.9993%, and the americium-naphthoium decontamination factor reached 10. 5 . Attached Figure Description

[0053] Figure 1 Preparation of dual-column circulation for the present invention 239 A schematic diagram of an Np tracer apparatus;

[0054] Figure 2 Used in Embodiment 1 of the present invention 243 Am and 239 γ-radioactivity spectrum of the original solution of Np parent-daughter body;

[0055] Figure 3 The product obtained by separation using Example 1 of the present invention 239 γ-radioactivity spectrum of Np tracer;

[0056] Figure 4 After separation using Example 1 of the present invention 243 The gamma radiometric spectrum of Am.

[0057] Attached reference numerals: 1-Feed solution storage tank, 2-Washing solution storage tank, 3-First-stage rinsing solution storage tank, 4-Second-stage rinsing solution storage tank, 5-Third-stage rinsing solution storage tank, 6-Product collector, 7-Waste liquid collector, 8-TODGA chromatography column, 9-LN or P 204 or P 50710-Valve, 11-Transfer pump, 12-Thermostat, 13-Radiation shield. Detailed Implementation

[0058] The present invention will now be described in further detail with reference to the accompanying drawings and specific embodiments.

[0059] like Figure 1 As shown, the dual-column cyclic preparation of the present invention 239 The Np tracer apparatus includes a temperature controller 12, a radiation shield 13, a liquid storage tank unit, a chromatography separation unit, a waste liquid collector 7, and a product collector 6. These units and devices are connected by piping, preferably silicone tubing. Corresponding valves 10 and a delivery pump 11 are installed within the piping. This allows for automatic control of the separation process via microcomputer control of the solenoid valves and peristaltic pump, reducing the impact of radionuclide radiation on the human body and lowering the workload of personnel. The peristaltic pump delivers the separation liquid using a flexible tube compression method, and the flow rate and velocity of the liquid are controlled by the pump's rotation speed.

[0060] The above-mentioned liquid storage tank unit includes a material liquid storage tank 1, a washing liquid storage tank 2, a first-stage rinsing liquid storage tank 3, a second-stage rinsing liquid storage tank 4, and a third-stage rinsing liquid storage tank 5. Each liquid storage tank is connected to the corresponding color layer adsorption column through valves and pumps, and realizes different functions.

[0061] The aforementioned chromatography separation unit includes a TODGA chromatography adsorption column 8, LN or P 204 or P 507 Chromatographic adsorption column 9.

[0062] The connection between the above-mentioned storage tanks and the chromatography column is as follows: the material storage tank 1 is located at the bottom, and its bottom end is connected to the inlet of the delivery pump through pipes and valves; the washing liquid storage tank 2, the first-stage rinsing liquid storage tank 3, the second-stage rinsing liquid storage tank 4, and the third-stage rinsing liquid storage tank 5 are arranged side by side at the top, and their outlets are connected to the inlet of the delivery pump 11 through valve 10; the outlet of the delivery pump 11 is connected to the TODGA chromatography column 8 and LN or P through valve 10 respectively. 204 or P 507 The inlet of the chromatography column 9 is connected; the outlet of the TODGA chromatography column 8 is connected to the waste liquid collector 7, LN or P via valve 10. 204 or P 507 The inlet of the chromatography adsorption column 9 and the product collector 6 are connected; LN or P 204 or P 507 The outlet of the color layer adsorption column 9 is connected to the waste liquid collector 7 and the liquid storage tank 1 via valve 10.

[0063] The separation steps of this invention are as follows:

[0064] Step 1: Preparation before separation

[0065] Add 100 mg of sodium nitrite to the radioactive solution containing americium-neptunium, keep it at a constant temperature of 70-100 degrees Celsius for 15 minutes, and then cool it to form the feed solution before separation; dissolve the acid in water to form an aqueous washing solution and an aqueous rinsing solution; the acid used is nitric acid and hydrochloric acid, hydrofluoric acid or a combination of the above acids, and the concentration of the acid is 0.01 to 8.0 mol / L; use a 4 mol / L to 8 mol / L HNO3 solution as the washing solution and place the washing solution in the washing solution storage tank (2); use a 0.01 mol / L to 0.5 mol / L HNO3 solution as the first-stage rinsing solution and place the first-stage rinsing solution in the first-stage rinsing solution storage tank (3); use a 0.05 mol / L to 0.2 mol / L HCl solution as the second-stage rinsing solution and place the second-stage rinsing solution in the second-stage rinsing solution storage tank (4); use a 0.05 mol / L to 0.5 ... The 0.05 mol / L to 0.2 mol / L HCl solution of HF is used as the third-stage eluent. The third-stage eluent is placed in the third-stage eluent storage tank (5); TODGA, LN or P are added. 204 or P 507 The resins were separately filled into the color layer columns.

[0066] TODGA chromatography columns are used to separate Np from Am and constant Na; LN or P 204 or P 507 Chromatographic columns are used to convert the acid system from the elution and recovery of Am into the americium-neptunium radioactive solution, achieving the required acid composition and concentration before column separation, so that it can be directly used for the next step. 239 Preparation of Np tracers.

[0067] Step 2: Using a peristaltic pump and a solenoid valve to pass the radioactive solution containing americium and neptunium through the TODGA chromatography column 8 for adsorption of americium and neptunium, the effluent is collected as waste liquid.

[0068] Step 3: Using a peristaltic pump and a solenoid valve to deliver the washing liquid through the TODGA chromatography column 8 for washing, adsorption and separation, the effluent is collected as waste liquid.

[0069] Step 4: Using a peristaltic pump and a solenoid valve, the first-stage eluent is passed through the TODGA chromatography column 8 for neptunium desorption; the effluent, i.e., the radioactive neptunium solution, is collected in the product collector 6.

[0070] Step 5: Using a peristaltic pump and a solenoid valve, the second-stage eluent is sequentially passed through the TODGA chromatography column 8 and LN or P. 204 or P 507The americium is desorbed and re-adsorbed using the chromatography column 9, and the effluent is collected as waste liquid.

[0071] Step 6: Using a peristaltic pump and a solenoid valve to allow the first-stage rinsing solution to pass through LN or P 204 or P 507 The chromatography adsorption column 9 is washed, and the effluent is collected as waste liquid.

[0072] Step 7: Use a peristaltic pump and a solenoid valve to allow the washing solution to pass through LN or P. 204 or P 507 The americium is desorbed by the chromatography adsorption column 9, and the effluent, i.e. the radioactive solution of americium, is collected in the americium-neptunium radioactive solution storage tank 1.

[0073] Step 8: Using a peristaltic pump and a solenoid valve, the third-stage eluent is passed through the TODGA chromatography column 8, and the effluent is collected as waste liquid.

[0074] Step 9: Using a peristaltic pump and a solenoid valve, deliver the second-stage rinsing solution through LN or P... 204 or P 507 The effluent from the pipeline between the chromatography adsorption column 9 and the TODGA chromatography adsorption column 8 is collected as waste liquid.

[0075] Step 10: Using a peristaltic pump and a solenoid valve, deliver the second-stage rinsing solution through LN or P... 204 or P 507 Chromatographic adsorption column 9, the effluent is collected as waste liquid;

[0076] Step 11: Using a peristaltic pump and a solenoid valve, the washing liquid is passed through the TODGA chromatography column 8, and the effluent is collected as waste liquid.

[0077] Step 12: After the americium solution in the americium-neptunium radioactive solution storage tank is left for 7-8 days, a sufficient amount of new americium will be generated. 239 Np, repeat steps one through eleven to begin the next preparation process, and repeat this cycle to prepare Np. 239 Np tracer.

[0078] In the above method, the radioactive solution of americium-neptunium is rich in sodium nitrite. 243 Am and its decay products 239 A solution composed of Np.

[0079] The specific implementation method is as follows:

[0080] Example 1

[0081] 100 mg of sodium nitrite was added to 15 mL of 5 mol / L HNO3 americium-neptunium radioactive solution placed in storage tank 1. The temperature was maintained at 80 degrees Celsius for 15 minutes using a temperature controller, followed by cooling to form the feed solution before separation. Its gamma-ray radioactivity spectrum is as follows: Figure 2 As shown.

[0082] The flow rate of the americium-containing solution was controlled at 1.5 mL / min, allowing the americium-containing solution to pass through a TODGA chromatography column 8 for separation. The TODGA chromatography column is... The TODGA chromatography column was used to separate americium and neptunium from the constant element Na, and the effluent was collected in waste liquid collector 7.

[0083] Use 15 mL of 5 mol / L HNO3 solution from the washing solution storage tank 2 to wash the TODGA chromatography adsorption column 8 at a flow rate of 2 mL / min. Collect the effluent in the waste liquid collector 7.

[0084] Neptunium was desorbed from the TODGA chromatography column 8 using 12 mL of 0.1 mol / L HNO3 solution from the first-stage eluent storage tank 3 at a flow rate controlled at 1.5 mL / min. The effluent, i.e., the radioactive solution of neptunium, was collected in the product collector 6, and its gamma-ray energy spectrum is as follows. Figure 3 As shown.

[0085] Using 15 mL of 0.1 mol / L HCl solution from the second-stage eluent storage tank 4, at a flow rate controlled at 1.5 mL / min, americium was desorbed and re-adsorbed sequentially through a TODGA chromatography column 8 and an LN chromatography column 8. The LN chromatography column was used for... An LN chromatography column was used to adsorb Am americium, and the effluent was collected as waste liquid.

[0086] Use 5 mL of 0.1 mol / L HNO3 solution from the first-stage rinsing solution storage tank 3, control the flow rate at 1.5 mL / min, and wash the solution through an LN chromatography adsorption column. Collect the effluent as waste liquid.

[0087] Americium was desorbed using an LN chromatography column by passing 15 mL of 5 mol / L HNO3 solution from washing solution storage tank 2 at a flow rate controlled at 1.5 mL / min. The effluent, i.e., the radioactive americium solution, was collected in storage tank 1 for the americium-neptunium radioactive solution. Its gamma-ray energy spectrum is shown below. Figure 4 As shown.

[0088] 10 mL of 0.1 mol / L HCl-0.3 mol / L HF solution was added to the third-stage eluent storage tank 5 and the flow rate was controlled at 1.5 mL / min. The solution was then passed through the TODGA chromatography adsorption column 8, and the effluent was collected as waste liquid.

[0089] Using 5 mL of 0.1 mol / L HCl solution from the second-stage eluent storage tank 4, and controlling the flow rate at 2 mL / min, the solution is passed through the pipeline between the LN chromatography column and the TODGA chromatography column 8, and the outflow is collected as waste liquid.

[0090] Use 15 mL of 0.1 mol / L HCl solution from the second-stage eluent storage tank 4, control the flow rate at 2 mL / min, and pass it through an LN chromatography adsorption column. Collect the effluent as waste liquid.

[0091] Use 15 mL of 5 mol / L HNO3 solution in the washing liquid storage tank 2, control the flow rate to 2 mL / min, and pass it through the TODGA chromatography adsorption column 8. Collect the effluent as waste liquid.

[0092] 239 Np and 243 The recovery rates of Am were 95.6% and 99.7%, respectively, and the separation process took 85 minutes. The neptunium product solution was left to stand for one month. 239 Np decays completely, identification 239 The Np radioactivity purity is 99.9993%.

[0093] Example 2

[0094] The americium-neptene radioactive solution storage tank in Example 1 243 After the Am solution was left to stand for 7 days, the separation process of Example 1 was repeated to obtain... 239 Np tracer and for use in the next cycle 243 Am solution. Measured 239 The Np recovery rate was 95.8%. 239 The Np radioactivity purity is 99.9992%. 243 The recovery rate of Am was 99.5%.

[0095] Example 3

[0096] The LN chromatography column in Example 1 was replaced with P. 204 Using a chromatography column, the separation process of Example 1 was repeated to obtain... 239 Np tracer and for use in the next cycle 243 Am solution. Measured 239 The recovery rate of the Np tracer was 95.1%. 239 The Np radioactivity purity is 99.9992%. 243 The recovery rate of Am was 99.4%. 239 The Np decontamination test determined that the decontamination factor of americium against neptunium was 1.3 × 10⁻⁶. 5 .

Claims

1. A dual-column circulation preparation method 239 The device for Np tracers is characterized in that, It includes a temperature controller (12), a radiation shield (13), a liquid storage tank unit, a color layer separation unit, a waste liquid collector (7), a product collector (6), a valve (10), and a transfer pump (11) assembly; The liquid in the storage tank unit enters the color separation unit via a transfer pump (11), and the liquid flowing out of the color separation unit enters the waste liquid collector (7), the product collector (6), or the material liquid storage tank (1); the components through which the liquid in the storage tank unit flows are connected by pipelines, and valves (10) are installed on the pipelines through which the liquid flows to each component. The liquid storage tank unit includes a material liquid storage tank (1), a washing liquid storage tank (2), a first-stage rinsing liquid storage tank (3), a second-stage rinsing liquid storage tank (4), and a third-stage rinsing liquid storage tank (5). Each liquid storage tank is connected to the color layer separation unit through a valve (10) and a delivery pump (11). The liquid storage tank (1) is located inside the temperature controller (12), and a radiation shield (13) is installed on the outside of the temperature controller (12); The color layer separation unit includes a TODGA color layer adsorption column (8), LN or P 204 or P 507 Chromatographic adsorption column (9); TODGA chromatography column (8) is used for the separation of Np from Am and macrosomal Na, LN or P. 204 or P 507 Chromatographic adsorption column (9) is used for rinsing and recovering americium; The connection relationship between the liquid storage tank unit and the color layer separation unit is as follows: the liquid storage tank (1) is placed at the lower end, and its bottom end is connected to the inlet of the delivery pump through pipelines and valves; the washing liquid storage tank (2), the first-stage rinsing liquid storage tank (3), the second-stage rinsing liquid storage tank (4) and the third-stage rinsing liquid storage tank (5) are placed side by side at the uppermost end. Its outlet is connected to the inlet of the transfer pump (11) via valve (10); the outlet of the transfer pump (11) is connected to the TODGA chromatograph column (8) and LN or P via valve (10) respectively. 204 or P 507 The inlet of the chromatography adsorption column (9) is connected; the outlet of the TODGA chromatography adsorption column (8) is connected to the waste liquid collector (7), LN or P through valve (10). 204 or P 507 The inlet of the chromatography adsorption column (9) and the product collector (6) are connected; LN or P 204 or P 507 The outlet of the color layer adsorption column (9) is connected to the waste liquid collector (7) and the liquid storage tank (1) respectively through the valve (10).

2. The dual-column circulation preparation method according to claim 1 239 The device for Np tracers is characterized in that, The tubing is made of silicone.

3. The dual-column circulation preparation method according to claim 1 239 The device for Np tracers is characterized in that, It also includes microcomputers, The microcomputer is used to control the valve (10) and the delivery pump (11); The valve (10) is a solenoid valve, and the delivery pump (11) is a peristaltic pump; the rotational speed of the peristaltic pump controls the flow rate and velocity of the liquid.

4. A dual-column circulation preparation method 239 The method using Np tracers is characterized by... Includes the following steps: Step 1, Preparation before separation: The radioactive solution of americium-neptunium to be separated was placed into the liquid storage tank (1), sodium nitrite was added, and the temperature of the liquid storage tank (1) was controlled by the temperature controller (12) to be 70℃~100℃. The temperature was kept for 15 minutes and then cooled to room temperature to obtain americium-neptunium-containing liquid. Using a 4 mol / L to 8 mol / L HNO3 solution as the washing liquid, the washing liquid is placed in the washing liquid storage tank (2); using a 0.01 mol / L to 0.5 mol / L HNO3 solution as the first-stage rinsing liquid, the first-stage rinsing liquid is placed in the first-stage rinsing liquid storage tank (3); Using a solution containing 0.05 mol / L to 0.2 mol / L HCl as the second-stage rinsing solution, the second-stage rinsing solution was placed in the second-stage rinsing solution storage tank (4); Using a 0.05mol / L to 0.2mol / L HCl solution containing 0.05mol / L to 0.5mol / L HF as the third-stage rinsing solution, the third-stage rinsing solution is placed in the third-stage rinsing solution storage tank (5); TODGA, LN, P 204 P 507 The resins were packed into color layer columns to obtain the corresponding color layer adsorption columns; Step two, adsorption of americium-neptunium: The liquid in the liquid storage tank (1) passes through the TODGA color layer adsorption column (8), so that americium and neptunium are adsorbed in the TODGA color layer adsorption column (8), and the effluent from the TODGA color layer adsorption column (8) is collected into the waste liquid collector (7). Step 3, Washing: The washing liquid in the washing liquid storage tank (2) is washed by the TODGA color layer adsorption column (8), and the effluent from the TODGA color layer adsorption column (8) is collected into the waste liquid collector (7). Step 4, Rinse: First, the first-stage rinsing solution in the first-stage rinsing solution storage tank (3) is rinsed through the TODGA chromatography column (8), and the effluent from the TODGA chromatography column (8) is collected in the product collector (6) to obtain a neptunium radioactive solution. Secondly, the second-stage eluent in the second-stage eluent storage tank (4) is passed sequentially through a TODGA chromatography column (8) and an LN or P column. 204 or P 507 Chromatographic adsorption column (9) is used for the desorption and re-adsorption of americium, LN or P. 204 or P 507 The effluent from the chromatography adsorption column (9) is collected in the waste liquid collector (7); Secondly, the first-stage rinsing solution passes through LN or P 204 or P 507 The effluent from the chromatography adsorption column (9) is collected in the waste liquid collector (7); Finally, the washing liquid in the washing liquid storage tank (2) is passed through LN or P 204 or P 507 Chromatographic adsorption column (9) is used for americium desorption, to remove LN or P 204 or P 507 The effluent from the chromatography adsorption column (9) is collected in the feed liquid storage tank (1).

5. The dual-column circulation preparation according to claim 4 239 The method using Np tracers is characterized by... It also includes step five, regeneration, the specific process of which is: First, the third-stage rinsing liquid in the third-stage rinsing liquid storage tank (5) passes through the TODGA chromatography adsorption column (8), and the effluent from the TODGA chromatography adsorption column (8) is collected into the waste liquid collector (7). Secondly, the second-stage rinsing solution in the second-stage rinsing solution storage tank (4) passes through LN or P 204 or P 507 The pipeline between the chromatography adsorption column (9) and the TODGA chromatography adsorption column (8) flows into the waste liquid collector (7); Next, the second-stage rinsing solution in the second-stage rinsing solution storage tank (4) is passed through LN or P 204 or P 507 Chromatographic adsorption column (9), for LN or P 204 or P 507 The effluent from the chromatographic adsorption column (9) is collected into the waste liquid collector (7); finally, the washing liquid in the washing liquid storage tank (2) passes through the TODGA chromatographic adsorption column (8), and the effluent from the TODGA chromatographic adsorption column (8) is collected into the waste liquid collector (7).

6. The dual-column circulation preparation according to claim 4 239 The method using Np tracers is characterized by... The amount of HNO3 in the americium-containing solution is 4 mol / L to 8 mol / L.

7. The dual-column circulation preparation according to claim 4 239 The method using Np tracers is characterized by... In the preparation before separation in step one, the americium radioactive solution to be separated is 15 mL of americium radioactive solution containing 5 mol / L HNO3, 100 mg of sodium nitrite is added, and the temperature of the liquid storage tank (1) is controlled by a temperature controller (12) to keep the temperature of the liquid storage tank (1) at 80°C. In step two, the adsorption of americium-neptunium, the flow rate of the feed solution is 1.5 mL / min, and the feed solution passes through a TODGA chromatography column (8). The TODGA chromatography column (8) is... In the washing process of step three, the washing solution is 15 mL of 5 mol / L HNO3 solution, the flow rate is 2 mL / min, and the washing solution is passed through a TODGA chromatography adsorption column (8). In step four, the first eluent is 12 mL of 0.1 mol / L HNO3 solution at a flow rate of 1.5 mL / min, passed through a TODGA chromatography column (8); in the second eluent, the second eluent is 15 mL of 0.1 mol / L HCl solution at a flow rate of 1.5 mL / min, passed through both the TODGA chromatography column (8) and the LN chromatography column for americium desorption and resorption. The LN chromatography column is... In the fourth step, the first-stage elution solution is 5 mL of 0.1 mol / L HNO3 solution at a flow rate of 1.5 mL / min, which is passed through an LN chromatography adsorption column. In the final step of the fourth step, the washing solution is 15 mL of 5 mol / L HNO3 solution at a flow rate of 1.5 mL / min, which is passed through an LN chromatography adsorption column for americium desorption.

8. The dual-column circulation preparation according to claim 5 239 The method using Np tracers is characterized by... In step five, the third-stage eluent is 10 mL of 0.1 mol / L HCl-0.3 mol / L HF solution, with a flow rate of 1.5 mL / min, which is passed through a TODGA chromatography adsorption column (8). In the second step of the fifth process, the second-stage elution solution is 5 mL of 0.1 mol / L HCl solution, with a flow rate of 2 mL / min; it passes through the pipeline between the LN chromatography column and the TODGA chromatography column (8); In step five, the second-stage eluent is 15 mL of 0.1 mol / L HCl solution at a flow rate of 2 mL / min, and the second-stage eluent is passed through an LN chromatography column. In the final step of step five, the washing solution is 15 mL of 5 mol / L HNO3 solution, the flow rate is 2 mL / min, and the washing solution is passed through a TODGA chromatography adsorption column (8).

9. The dual-column circulation preparation according to claim 4 239 The method using Np tracers is characterized by... The americium-neptunium radioactive solution is rich in sodium nitrite. 243 Am and its decay products 239 A solution composed of Np.

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